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Modulating Hydrogen Exchange Capabilities by Heterogenizing Pd Nanoclusters onto Ni3C Multipods for Efficiently
Zulakha Zafar1, Bin Zhao1, Rida Javed1
1College of Civil and Transportation Engineering, College of Materials Science and Engineering, Shenzhen Key Laboratory of Energy Electrocatalytic Materials, Guangdong Provincial Key Laboratory of New Energy Materials Service Safety, Shenzhen University, Shenzhen 518055, China.
This study introduces a novel nickel-based catalyst for converting industrial pollutants nitrate and formaldehyde into valuable products like ammonia and hydrogen, while also generating electricity. This bifunctional catalyst offers an efficient and sustainable solution for waste remediation and energy production.
Area of Science:
- Electrochemistry
- Materials Science
- Environmental Science
Background:
- Nitrate and formaldehyde are hazardous industrial pollutants requiring efficient conversion methods.
- Existing coupled nitrate reduction (NO3RR) and formaldehyde oxidation (FOR) strategies face limitations like lack of H2 generation, no electricity output, and reliance on deactivating Cu catalysts.
- Developing non-copper, bifunctional catalysts with enhanced H* transfer is crucial for efficient dual-directional catalysis.
Purpose of the Study:
- To develop a non-copper bifunctional catalyst for simultaneous NO3RR and FOR.
- To investigate the catalyst's performance in generating valuable chemicals and electricity from industrial waste.
- To elucidate the reaction mechanism, particularly H2 evolution during formaldehyde oxidation.
Main Methods:
- Synthesis of palladium nanoclusters on nickel carbide (Pdnc-Ni3C).
- Electrochemical characterization of NO3RR and FOR performance, including onset potentials and Faradaic efficiencies.
- Differential electrochemical mass spectrometry (DEMS) for mechanistic studies.
- Assembly and testing of a formaldehyde-nitrate galvanic cell.
Main Results:
- Pdnc-Ni3C demonstrated superior H* exchange capabilities for dual-directional catalysis.
- Efficient NO3RR with 98% NH3 Faradaic efficiency at -0.3 V and efficient FOR at a low onset potential of 0.04 V.
- A formaldehyde-nitrate galvanic cell achieved an open-circuit voltage (OCV) of 0.88 V and peak power density of 7.4 mW cm-2.
- Identified a novel intermolecular coupling pathway for H2 evolution during formaldehyde oxidation.
Conclusions:
- The Pdnc-Ni3C catalyst effectively converts industrial waste (nitrate, formaldehyde) into green energy carriers (H2, NH3) and value-added chemicals (formate).
- This Ni-based system simultaneously produces electricity, offering significant environmental and economic benefits.
- The study advances mechanistic understanding of formaldehyde oxidation and H2 evolution, paving the way for improved catalytic systems.
